CN113680394B - Treatment method of uranium-containing waste strong base anion exchange resin - Google Patents
Treatment method of uranium-containing waste strong base anion exchange resin Download PDFInfo
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- CN113680394B CN113680394B CN202110993841.7A CN202110993841A CN113680394B CN 113680394 B CN113680394 B CN 113680394B CN 202110993841 A CN202110993841 A CN 202110993841A CN 113680394 B CN113680394 B CN 113680394B
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J49/00—Regeneration or reactivation of ion-exchangers; Apparatus therefor
- B01J49/40—Thermal regeneration
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J49/00—Regeneration or reactivation of ion-exchangers; Apparatus therefor
- B01J49/50—Regeneration or reactivation of ion-exchangers; Apparatus therefor characterised by the regeneration reagents
- B01J49/57—Regeneration or reactivation of ion-exchangers; Apparatus therefor characterised by the regeneration reagents for anionic exchangers
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/42—Treatment of water, waste water, or sewage by ion-exchange
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/42—Treatment of water, waste water, or sewage by ion-exchange
- C02F2001/422—Treatment of water, waste water, or sewage by ion-exchange using anionic exchangers
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/006—Radioactive compounds
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2303/00—Specific treatment goals
- C02F2303/14—Maintenance of water treatment installations
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P10/00—Technologies related to metal processing
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- Environmental & Geological Engineering (AREA)
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- Treatment Of Water By Ion Exchange (AREA)
- Processing Of Solid Wastes (AREA)
Abstract
The invention provides a treatment method of uranium-containing waste strong base anion exchange resin, belonging to the technical field of solid waste treatment. The invention heats and mixes uranium-containing waste strong base anion exchange resin with soluble carbonate and water. Because the strong base anion exchange resin has quaternary ammonium ion exchange functional groups, after uranium is adsorbed by an ion exchange mode, a quaternary ammonium-uranyl ion complex is formed, and under the heating condition, the quaternary ammonium groups containing uranyl ions can be subjected to Hofman degradation and fall off from the resin. In addition, the uranium-containing waste strong base anion exchange resin is treated by utilizing the characteristics of strong base anion exchange resin that the uranium-containing waste strong base anion exchange resin is degraded by heating and the uranium-containing waste strong base anion exchange resin and carbonate are easy to complex, so that the uranium content in the waste resin can be effectively reduced, the radioactivity of the waste strong base anion exchange resin is less than 1Bq/g of dry resin, the level of exemption is reached, and the waste resin can be treated according to general waste.
Description
Technical Field
The invention relates to the technical field of solid waste treatment, in particular to a treatment method of uranium-containing waste strong base anion exchange resin.
Background
In nature, natural uranium is mostly treated with uranyl ions (UO 2 2+ ) Is present. The extraction of natural uranium in uranium mining and metallurgy facilities mainly utilizes sulfate to leach uranium in the ore, formed uranium complex anions are selectively adsorbed by strong alkali anion exchange resin, and then the uranium complex is leached from the resin by using a leaching agent, so that the purification and concentration of the natural uranium are realized.
In uranium smelting facilities, the use amount of the strong alkali anion exchange resin is large, a large amount of radioactive strong alkali anion exchange resin containing natural uranium is left after the uranium smelting facilities are retired, and the content of uranium in waste resin is generally 0.1-1 mg/g of dry resin. The radioactivity of the waste strong base anion exchange resins is more than 1Bq/g, and the waste strong base anion exchange resins cannot be treated according to the exemption and can only be placed into a tailing pond for landfill treatment.
Because the volume of the strong base anion exchange resin expands after water absorption, if a large amount of waste strong base anion exchange resin enters the tailing pond and then influences the stability of the tailing pond, the waste strong base anion exchange resin of uranium mining and metallurgy facilities is necessarily treated to reach an exemption level, and then is treated according to general waste.
Disclosure of Invention
In view of the above, the invention aims to provide a treatment method of uranium-containing waste strong base anion exchange resin. The treatment method can effectively reduce the uranium content in the uranium-containing waste strong base anion exchange resin, so that the waste strong base anion exchange resin reaches the exemption level.
In order to achieve the above object, the present invention provides the following technical solutions:
the invention provides a treatment method of uranium-containing waste strong base anion exchange resin, which comprises the following steps:
heating and mixing uranium-containing waste strong base anion exchange resin with soluble carbonate and water.
Preferably, the soluble carbonate is one or more of sodium carbonate, potassium carbonate, sodium bicarbonate, ammonium carbonate and ammonium bicarbonate.
Preferably, the mass ratio of the soluble carbonate to the water is 2-20:1000.
Preferably, the mass ratio of the uranium-containing waste strong base anion exchange resin to water is 1:3-10.
Preferably, the temperature of the heating and mixing is 60-100 ℃.
Preferably, the heating and mixing time is 2-72 h.
Preferably, the uranium content in the uranium-containing waste strong base anion exchange resin is less than or equal to 1mg/g dry resin.
Preferably, after the heating and mixing, the solid-liquid separation is further performed on the mixture, and the obtained solid is dried.
The invention provides a treatment method of uranium-containing waste strong base anion exchange resin, which comprises the following steps: heating and mixing uranium-containing waste strong base anion exchange resin with soluble carbonate and water. The strong base anion exchange resin has quaternary ammonium ion exchange functional groups, and the quaternary ammonium-uranyl ion complex is formed after uranium is adsorbed in an ion exchange mode. Under the heating condition, the quaternary ammonium group containing uranyl ions can be subjected to Hofman degradation and fall off from the resin. In addition, uranyl ions and carbonate have strong complexing ability. According to the invention, the uranium-containing waste strong base anion exchange resin is treated by utilizing the characteristics of thermal degradation of the strong base anion exchange resin and easiness in complexing of uranyl ions and carbonate, so that the uranium content in the uranium-containing waste strong base anion exchange resin can be effectively reduced, and the waste strong base anion exchange resin reaches the exemption level. The results of the examples show that the resin treated according to the invention has a radioactivity of less than 1Bq/g dry resin and can be disposed of as normal waste.
Detailed Description
The invention provides a treatment method of uranium-containing waste strong base anion exchange resin, which comprises the following steps:
heating and mixing uranium-containing waste strong base anion exchange resin with soluble carbonate and water.
As one embodiment of the invention, the structural formula of the strong base anion exchange resin is shown in the formula 1.
Because the bond energy and the decomposition activation energy of the quaternary ammonium ions of the strong base anion exchange resin are lower, hofman degradation of the strong base group can occur at a higher temperature (more than 60 ℃), the strong base group falls off or is degraded into weak base resin, the strong base exchange function of the resin is finally reduced, and even the strong base exchange capability is lost, and the use temperature of the strong base anion exchange resin is not more than 60 ℃. Because the strong base anion exchange resin has quaternary ammonium ion exchange functional groups, the quaternary ammonium-uranyl ion complex is formed after uranium is adsorbed in an ion exchange mode. Under the heating condition, the quaternary ammonium group containing uranyl ions can be subjected to Hofman degradation and fall off from the resin. In addition, uranyl ions and carbonate have strong complexing ability. According to the invention, the uranium-containing waste strong base anion exchange resin is treated by utilizing the characteristics of thermal degradation of the strong base anion exchange resin and easiness in complexing of uranyl ions and carbonate, so that the uranium content in the uranium-containing waste strong base anion exchange resin can be effectively reduced, and the waste strong base anion exchange resin reaches the exemption level.
The uranium-containing waste strong base anion exchange resin has no special requirement, and the uranium-containing waste strong base anion exchange resin well known in the art can be subjected to uranium removal treatment by using the method provided by the application. In the invention, the uranium-containing waste strong alkali anion exchange resin is preferably generated after uranium ore smelting facilities are retired. In the invention, the uranium content in the uranium-containing waste strong base anion exchange resin is preferably 0.1-1 mg/g dry resin, more preferably 0.2-0.8 mg/g dry resin.
In the invention, the soluble carbonate is one or more of sodium carbonate, potassium carbonate, sodium bicarbonate, ammonia carbonate and ammonia bicarbonate. In the present invention, the water is preferably deionized water.
In the present invention, the mass ratio of the soluble carbonate to water is preferably 2 to 20:1000, more preferably 5 to 15:1000, and even more preferably 8 to 10:1000.
In the present invention, the mixing means is preferably: mixing the soluble carbonate with water to obtain a soluble carbonate aqueous solution; heating and mixing uranium-containing waste strong base anion exchange resin with soluble carbonate aqueous solution.
In the present invention, the mass concentration of the soluble carbonate aqueous solution is preferably 2 to 20g/L, more preferably 5 to 15g/L, and still more preferably 8 to 10g/L.
In the invention, the volume ratio of the mass of the uranium-containing waste strong base anion exchange resin to water is preferably 1:3-10, and more preferably 1:8.
In the present invention, the heating and mixing are preferably performed under stirring. In the present invention, the temperature of the heating and mixing is preferably 60 to 100 ℃, more preferably 90 to 100 ℃; the heating and mixing time is preferably 2 to 72 hours, more preferably 10 to 20 hours. In the present invention, the heating rate to the heating and mixing temperature is preferably 5 to 10 ℃/min. The invention calculates the time of heating and mixing after the temperature reaches the temperature of the heating and mixing.
In the present invention, after the heating and mixing, the present invention preferably performs solid-liquid separation of the resultant mixture. The specific operation mode of the solid-liquid separation is not particularly required, and the solid-liquid separation mode known by the person skilled in the art can be used, such as filtration.
In the invention, after the solid-liquid separation, the obtained solid is preferably dried to obtain the reprocessed waste strong base anion exchange resin. In the present invention, the drying temperature is preferably 80 to 100 ℃, more preferably 90 ℃, and the time is preferably 2 to 3 hours. In the invention, the uranium content in the obtained reprocessed waste strong base anion exchange resin is preferably less than or equal to 0.015mg/g of dry resin, the radioactivity is less than 1Bq/g of dry resin, the method accords with the exemption level of the standard GB18871-20002 of basic Standard for electric radiation protection and radiation source safety, and the reprocessed waste anion exchange resin can be treated according to general waste.
In the invention, after the solid-liquid separation, the obtained liquid is uranium-containing waste liquid, and is treated in a lime precipitation mode.
The following describes the treatment method of uranium-containing waste strong base anion exchange resin provided in the present invention in detail with reference to examples, but they should not be construed as limiting the scope of the present invention.
In the following embodiment, the method for testing the uranium content in the uranium-containing waste strong base anion exchange resin is a microwave digestion resin, so that natural uranium in the resin enters an aqueous solution, and then the content of the natural uranium in water is analyzed.
Example 1
10g of sodium carbonate and 200mL of deionized water are added into a 500mL three-port bottle with a stirring paddle and a thermometer, 25g of uranium-containing waste 201X 7 strong base anion exchange resin is added, the content of uranium in the waste resin is 0.2mg/g of dry resin, the temperature is raised to 90 ℃, and stirring reaction is carried out for 24 hours.
After the reaction is finished, the uranium content in the waste resin is measured to be 0.02mg/g dry resin, the radioactivity is less than 1Bq/g dry resin, and the radioactive waste exemption level is reached.
Example 2
15g of sodium carbonate and 200mL of deionized water are added into a 500mL three-port bottle with a stirring paddle and a thermometer, 25g of uranium-containing waste 201X 7 strong base anion exchange resin is added, the content of uranium in the waste resin is 0.2mg/g of dry resin, the temperature is raised to 95 ℃, and stirring reaction is carried out for 14 hours.
After the reaction is finished, the uranium content in the resin is measured to be 0.015mg/g dry resin, and the radioactivity is less than 1Bq/g dry resin, so that the radioactive waste exemption level is reached.
Example 3
Adding 20g of sodium carbonate into a 500mL three-port bottle with a stirring paddle and a thermometer, heating 200mL of deionized water, adding 25g of uranium-containing waste 201X 7 strong base anion exchange resin, heating to 100 ℃ and stirring for reaction for 10 hours, wherein the uranium content in the waste resin is 0.2mg/g of dry resin.
After the reaction is finished, the uranium content in the resin is measured to be 0.03mg/g dry resin, the radioactivity is less than 1Bq/g dry resin, and the radioactive waste exemption level is reached.
The foregoing is merely a preferred embodiment of the present invention and it should be noted that modifications and adaptations to those skilled in the art may be made without departing from the principles of the present invention, which are intended to be comprehended within the scope of the present invention.
Claims (4)
1. A treatment method of uranium-containing waste strong base anion exchange resin comprises the following steps:
heating and mixing uranium-containing waste strong base anion exchange resin with soluble carbonate and water;
the structural formula of the strong base anion exchange resin is shown as formula 1;
the mass ratio of the soluble carbonate to the water is 2-20:1000;
the mass ratio of the uranium-containing waste strong base anion exchange resin to water is 1:3-10;
the temperature of the heating and mixing is 90-100 ℃;
the heating and mixing time is 2-72 h.
2. The process of claim 1, wherein the soluble carbonate is one or more of sodium carbonate, potassium carbonate, sodium bicarbonate, ammonium carbonate and ammonium bicarbonate.
3. The method according to claim 1, wherein the uranium content in the uranium-containing waste strong base anion exchange resin is not more than 1mg/g dry resin.
4. The method according to claim 1, wherein the heating and mixing further comprises subjecting the mixture to solid-liquid separation, and drying the obtained solid.
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| Application Number | Priority Date | Filing Date | Title |
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| CN202110993841.7A CN113680394B (en) | 2021-08-27 | 2021-08-27 | Treatment method of uranium-containing waste strong base anion exchange resin |
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| CN202110993841.7A CN113680394B (en) | 2021-08-27 | 2021-08-27 | Treatment method of uranium-containing waste strong base anion exchange resin |
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| CN113680394B true CN113680394B (en) | 2023-07-25 |
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Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB910025A (en) * | 1958-03-06 | 1962-11-07 | Commissariat Energie Atomique | Improvements in methods for the alkaline treatment of uranium ores by means of ion exchange resins |
| US4280985A (en) * | 1979-03-16 | 1981-07-28 | Mobil Oil Corporation | Process for the elution of ion exchange resins in uranium recovery |
| US4397819A (en) * | 1980-12-31 | 1983-08-09 | Mobil Oil Corporation | Rejuvenation of the anion exchanger used for uranium recovery |
| US4430308A (en) * | 1982-12-13 | 1984-02-07 | Mobil Oil Corporation | Heated ion exchange process for the recovery of uranium |
| AU1058783A (en) * | 1983-01-19 | 1984-07-26 | Mobil Oil Corp. | Regenerating ion-exchangers used in uranium recovery |
| CA1203081A (en) * | 1982-12-31 | 1986-04-15 | Raymond J. Jan | Process for the separation and recovery of molybdenum and uranium from leach solution using ion exchange |
-
2021
- 2021-08-27 CN CN202110993841.7A patent/CN113680394B/en active Active
Patent Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB910025A (en) * | 1958-03-06 | 1962-11-07 | Commissariat Energie Atomique | Improvements in methods for the alkaline treatment of uranium ores by means of ion exchange resins |
| US4280985A (en) * | 1979-03-16 | 1981-07-28 | Mobil Oil Corporation | Process for the elution of ion exchange resins in uranium recovery |
| US4397819A (en) * | 1980-12-31 | 1983-08-09 | Mobil Oil Corporation | Rejuvenation of the anion exchanger used for uranium recovery |
| US4430308A (en) * | 1982-12-13 | 1984-02-07 | Mobil Oil Corporation | Heated ion exchange process for the recovery of uranium |
| CA1203081A (en) * | 1982-12-31 | 1986-04-15 | Raymond J. Jan | Process for the separation and recovery of molybdenum and uranium from leach solution using ion exchange |
| AU1058783A (en) * | 1983-01-19 | 1984-07-26 | Mobil Oil Corp. | Regenerating ion-exchangers used in uranium recovery |
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